A novel iridium/acid co-catalysed transfer hydrogenative coupling strategy, enabling direct alkylation of C(sp3)–H bonds and atom-economic access to alkyl chain-lengthened N-heteroaromatics from six-membered 2-alkyl cyclic amines and aldehydes, has been demonstrated. This work has built an important basis to convert cyclic amines, a class of bulk chemical raw materials, into functionalized products.
